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CN112118906B - Hydrocarbon trap catalyst - Google Patents

Hydrocarbon trap catalyst Download PDF

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Publication number
CN112118906B
CN112118906B CN201980032971.5A CN201980032971A CN112118906B CN 112118906 B CN112118906 B CN 112118906B CN 201980032971 A CN201980032971 A CN 201980032971A CN 112118906 B CN112118906 B CN 112118906B
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catalyst
palladium
length
substrate
zeolite
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CN112118906A (en
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J·G·努南
D·H·莫泽
C·埃尔泰泽尔
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Umicore AG and Co KG
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Umicore AG and Co KG
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Abstract

The invention relates to a catalyst comprising a carrier substrate of length L extending between substrate ends a and B and two washcoat zones a and B, wherein washcoat zone a comprises a redox active alkali metal and palladium supported on a zeolite and/or refractory oxide support and extends over a part of length L starting from substrate end a, and washcoat zone B comprises the same components and additional amounts of palladium as washcoat a and extends over a part of length L from substrate end B, wherein l=l A +L B Wherein L is A Length of the wash coat zone A and L B Is the length of the substrate length B.

Description

Hydrocarbon trap catalyst
The present invention relates to a hydrocarbon trapping catalyst for trapping hydrocarbons during a cold start of a combustion engine operating at a predominantly stoichiometric air/fuel ratio.
It is well known in the combustion engine art that fuel combustion is incomplete and therefore produces pollutant emissions such as unburned Hydrocarbons (HC), carbon monoxide (CO), nitrogen oxides (NO x ) And Particulate Matter (PM). To improve air quality, emission limits regulations are enacted to achieve low emissions of pollutants for stationary applications and mobile sources. For mobile sources such as passenger cars, active strategies such as improving combustion and optimizing a/F or lambda control have been implemented in an effort to reduce pollutant emissions. Improving fuel-air mixing (a/F ratio) as a primary measure substantially reduces pollutants. However, the use of heterogeneous catalysts has become unavoidable since more stringent regulations have been imposed over the years.
For gasoline engines, so-called Three Way Catalysts (TWCs) are capable of eliminating HC, CO and NO x . The use of TWCs is optimal in the vicinity of λ=1± -0.005, i.e. the air/fuel ratio is equal to 14.56. Above these values, the exhaust gas is said to be lean and contains an excess of an oxidant such as O 2 And NOx, and CO and HC are catalytically oxidized to carbon dioxide and water. Below this value, the exhaust gas is said to be rich and contains excess reductant such as H 2 CO and HC, and uses, for example, CO as a reducing agent to predominantly NO x Reducing to nitrogen.
Achieving HC, CO and NO when λ=1 x Is used for the conversion of the catalyst. However, gasoline engines operate under oscillating conditions, i.e. between slightly lean and slightly rich conditions. Under pure enrichment conditions in which the TWC is operated, oxygen Storage Materials (OSM) in the form of cerium-zirconium mixed oxides are included in the formulation of the TWC.
Like other catalysts, three-way catalysts are inactive until a certain temperature is reached (the so-called light-off temperature, which is typically about 200 ℃). Below this temperature, for example during a cold start, other measures need to be taken to avoid escape of pollutants via the exhaust pipe. This is particularly important in terms of hydrocarbons, as they are mainly produced during cold starts.
This has led to the development of so-called hydrocarbon traps. HC traps are basically storage materials that adsorb hydrocarbons when the exhaust gas is cooled and the three-way catalyst has not been activated (e.g., during a cold start), and desorb and release hydrocarbons when the exhaust gas temperature is higher and the three-way catalyst has reached its light-off temperature.
The material used for storing hydrocarbons is typically a zeolite material or a so-called molecular sieve. Examples are Mordenite (MOR), Y-zeolite (FAU), ZSM-5 (MFI), beta-zeolite (BEA), and mixtures thereof, for example. These zeolites are preferably in the H-form or NH 4 The form is used or exchanged with a transition metal.
The catalytic HC-trap integrates an oxidation function into a storage function and preferably consists of an adsorbent material containing a zeolite material and a three-way catalyst containing an oxygen storage component and platinum group metals such as platinum, palladium and rhodium, for example in the form of separate layers. In many designs, the sorbent layer is positioned to be applied to the bottom or first layer of the support substrate, and the TWC serves as the second or top overcoat layer. This allows the hydrocarbons desorbed and released by the adsorbent material to be directly oxidized.
Oxidation may be achieved by oxygen present in the gas phase or oxygen from an "oxygen carrier" in the trap washcoat (washcoat). The latter component may comprise a redox-active alkali metal such as those derived from oxides of transition metals (such as Fe, mn, co, ni and Cu), rare earth elements (such as Ce, pr, sm, tb) or P-block elements (such as Sn and In).
In standard TWC designs, the Platinum Group Metals (PGMs) are distributed uniformly over the entire length of the HC-trap substrate or localized into highly concentrated platinum group metal regions at the catalyst inlet relative to the exhaust flow direction.
In a typical HC trap application, the exhaust system consists of a tightly coupled TWC catalyst with the HC trap positioned as a separate converter in a cooled underframe position. In this type of application, the HC trap heats up slowly and has a large temperature gradient of up to 100deg.C between the front inlet end of the trap compared to the rear outlet. The hydrocarbons are initially adsorbed by the inlet end of the trap relative to the exhaust flow because they initially contact this location of the trap. As the trap heats up, the desorption/adsorption process occurs such that the adsorbed hydrocarbons move from the front to the back of the trap in a manner similar to the movement of solvent with optional other dissolved components in the chromatographic column, whereby the solvent and soluble components gradually move from the bottom of the column to higher levels. The molecules trapped in the hotter front region of the desorption trap are then quickly re-adsorbed by the cooler rear region of the trap until the adsorbed molecules gradually reach the rear section of the trap where they are eventually desorbed into the gas phase and escape the trap.
It has now been found that the location or arrangement of highly concentrated platinum group metals at the trap inlet is not the optimal strategy for zoning due to the adsorption-desorption method and the movement of the trapped hydrocarbons. This is because once adsorbed hydrocarbons move past the inlet zone on their way to the rear of the trap, any hydrocarbon conversion potential is lost. On the other hand, where a high platinum group metal zone is located at the rear of the trap, all adsorbed hydrocarbons must move through the zone and if the platinum group metal concentration is sufficiently high, conversion can occur.
The invention therefore relates to a catalyst comprising a carrier substrate of length L extending between substrate ends a and B and two washcoat zones A and B, wherein
The washcoat zone A comprises a compound of a redox-active alkali metal selected from Cu, ni, co, mn, fe, cr, ce, pr, tb, sn and In supported on zeolite and/or on a support oxide and palladium and extends over a portion of the length L from the substrate end a, and
the washcoat zone B comprises the same composition and additional amounts of palladium as the washcoat zone a and extends from the substrate end B over a portion of the length L,
wherein l=l A +L B Wherein L is A Length of the wash coat zone A and L B Is the length of the washcoat zone B.
Thus, according to the invention, the redox active alkali metal compound and the zeolite and/or support oxide are uniformly distributed over the entire length L of the carrier substrate, while palladium is present in the washcoat zone B in a higher concentration than in the washcoat zone a.
In one embodiment of the invention, the washcoat zone A comprises two layers A1 and A2, both of which are at length L A Upper extension, wherein layer A1 comprises a compound of a redox-active alkali metal selected from Cu, ni, co, mn, fe, cr, ce, pr, tb, sn and In supported on zeolite and/or on a support oxide, and palladium, said redox-active alkali metal and layer A2 comprises rhodium, and washcoat zone B comprises two layers B1 and B2, both layers being of length L B Upper extension, wherein layer B1 comprises the same composition as layer A1 and layer B2 comprises the same composition as layer A2, and wherein layers B1 and B2 comprise an additional amount of palladium compared to layers A1 and A2.
In an embodiment of the invention, layer A2 may comprise one or more additional platinum group metals in addition to rhodium, in particular platinum and palladium, preferably palladium. In the latter case, the weight ratio Pd: rh is, for example, from 10:1 to 1:10.
In a preferred embodiment of the present invention, washcoat zone A and B are identical except for a greater amount of palladium in washcoat zone B.
Also, layers A1 and B1 are identical except for a greater amount of palladium in layer B1, and layers A2 and B2 are identical except for a greater amount of palladium in layer B2.
Preferred redox-active alkali metals are copper, manganese and iron. A particularly preferred redox active alkali metal is iron.
In an embodiment of the invention, the redox-active alkali metal compound is present as a cation or as an oxide. If present in cationic form, a counterion must be present, which can be a zeolite. In other words, the metal cations are localized within the three-dimensional zeolite structure as ion-exchange species and neutralize their negative charge.
Alternatively or in addition, the redox-active alkali metal compound may be present in the form of an oxide in the case of iron, for example as Fe 2 O 3 And dispersed as finely dispersed metal oxide crystallites on the zeolite crystallites. In any case, the redox-active alkali metal compound may be present in the zeolite structure in cationic form or in the zeolite and/or on the surface of the zeolite in oxide form.
Based on the volume of the carrier substrate and calculated as metal oxide, in the case of iron being Fe 2 O 3 The redox active alkali metal compound is generally present in the washcoat zones A and B in an amount of from 1.0g/l to 30 g/l.
In the case of palladium supported on a zeolite, the zeolite preferably belongs to the structural type code (as defined in zeolite framework type catalogue, elsevier, sixth revision, 2007 (Atlas of Zeolite Framework Types, elsevier, sixth revised edition, 2007)) BEA, FAU, FER, MFI or MOR. Preferred zeolites belong to the structure type code BEA.
Preferred zeolites have SAR (silica to alumina ratio) values of from 2 to 100, in particular from 5 to 50.
The palladium in layers a and A1 may be present in the form of cations, metals or oxides, respectively, and is preferably present in the zeolite and/or on the surface of the zeolite.
The zeolite is generally present in the washcoat zones A and B in an amount of 120g/l to 340g/l based on the volume of the support substrate.
In the case where palladium is supported on a support oxide, suitable support oxides are alumina, silica, magnesia, titania, ceria, zirconia, and mixtures or mixed oxides comprising at least two of these materials.
Typically, they have a length of 30m 2 /g to 250m 2 /g, preferably 100m 2 /g to 200m 2 BET surface area per g (determined in accordance with German standard DIN 66132).
Preference is given to aluminum oxide, aluminum oxide/silicon dioxide mixed oxides and magnesium oxide/aluminum oxide mixed oxides. In the case of aluminum oxide, it is preferably stabilized, for example, with 1 to 6% by weight, in particular 4% by weight, of lanthanum oxide.
In particular, the preferred support oxide has oxygen storage properties and is, for example, ceria-zirconia mixed oxide or alumina-ceria mixed oxide.
Specifically, the support oxide is selected from the group consisting of alumina, alumina/silica mixed oxide, magnesia/alumina mixed oxide, ceria-zirconia mixed oxide, and alumina-ceria mixed oxide.
The support oxide in washcoat zone a and B is preferably present in an amount of 1.0 wt% to 50.0 wt% based on the weight of washcoat zone a and washcoat zone B.
Palladium is preferably immobilized to the surface of the support oxide in an oxidized or metallic state.
Palladium is generally present in washcoat zones a and A1, respectively, in an amount of 0.04g/l to 4.0g/l, based on the zone volume of the support substrate and calculated as rhodium metal.
The palladium content in washcoat zone B is higher than the palladium content in washcoat zone a and is typically from 2g/l to 20g/l, based on the zone volume of the support substrate and calculated as palladium metal.
The advantage of palladium over other platinum group metals (such as platinum and rhodium) is lower cost and in particular it is highly effective for burning hydrocarbons, especially large hydrocarbons (such as branched olefinic hydrocarbons/alkane hydrocarbons and aromatics) that will be retained in the trap to higher temperatures. In addition, with respect to palladium, there is a high performance gradient with respect to palladium loading and HC light-off. From 10g/ft after moderate to severe aging 3 The low Pd loading of (0.35 g/l) was shifted to justExceeding 100g/ft 3 At loadings of (3.5 g/l), the light-off temperature can be reduced by more than 100 ℃.
In the case where the catalyst of the present invention comprises washcoat layers A1 and A2 and layers B1 and B2, respectively, rhodium and optionally additional platinum group metals such as palladium contained in layers A2 and B2 are typically supported on a support material.
As support materials, all materials known to the person skilled in the art can be used. In general, they have BET surface areas of from 30m2/g to 250m2/g, preferably from 100m2/g to 200m2/g (determined in accordance with DIN 66132), and in particular aluminum oxide, silicon dioxide, magnesium oxide, titanium dioxide and mixtures or mixed oxides comprising at least two of these materials.
Preference is given to aluminum oxide, aluminum oxide/silicon dioxide mixed oxides and magnesium oxide/aluminum oxide mixed oxides. In the case of aluminum oxide, it is preferably stabilized, for example, with 1 to 6% by weight, in particular 4% by weight, of lanthanum oxide.
Rhodium is generally present in layers A2 and B2 in an amount of from 0.04g/l to 4.0g/l, based on the volume of the support substrate and calculated as rhodium metal.
In an embodiment of the invention, the washcoat zone a extends over 70% to 95%, preferably 73% to 90% of the length L of the carrier substrate and the washcoat zone B extends over 5% to 30%, preferably 10% to 27% of the length L of the carrier substrate.
In embodiments of the invention, the length L of the carrier substrate may be a flow-through substrate or a filtration substrate. Such carrier substrates are typically made of cordierite or metal and are described in the literature and are commercially available.
The catalysts of the invention can be manufactured by known processes, in particular by a two-stage process, comprising:
coating the carrier substrate with a coating suspension (wash coat) containing the components of the wash coat zone A over the entire length L of the carrier substrate, and
immersing the coated support substrate in an aqueous solution containing a water-soluble palladium compound to a length corresponding to the length of the washcoat zone B so as to form the washcoat zone B.
The coating in the first step is typically carried out via conventional dipping, suction and pumping methods, which are widely described in the literature and known to those skilled in the art.
The first and second steps are typically followed by calcination and optionally thermal reduction in an atmosphere containing a forming gas.
The catalyst of the present invention is suitable for treating exhaust gas of a combustion engine operating at a predominantly stoichiometric air/fuel ratio by passing the exhaust gas over the catalyst of the present invention.
The invention therefore also relates to a method for treating exhaust gas of an engine operating at a predominantly stoichiometric air/fuel ratio, characterized in that the exhaust gas passes through a catalyst according to the invention, wherein the exhaust gas enters the catalyst at a substrate end a and leaves the catalyst at a substrate end b.
Fig. 1 shows a catalyst according to the invention.
The upper part shows details of the catalyst (1) according to the invention, which catalyst (1) comprises a carrier substrate (3), which carrier substrate (3) extends between the substrate ends a and B and carries a washcoat zone a (4) and a washcoat zone B (5).
The lower part shows details of another embodiment of the invention. The catalyst (2) comprises a carrier substrate (3) extending between substrate ends a and b. The washcoat zone A includes layers A1 (6) and A2 (7), while the washcoat zone B includes layer B1 (9) and layer B2 (8). The layers A1 (6) and B1 (9) differ only in that B1 (9) contains a greater amount of palladium than A1 (6). Also, layers A2 (7) and B2 (8) differ only in that B2 (8) contains a greater amount of palladium than A2 (7).
Comparative example 1
a) Slurry preparation began with the addition of an alumina stabilized silica sol (Aeroperl 3375/20 from Evonik) to water and mixing. This material represents 4.5 wt% of the final calcined washcoat loading. After this step, boehmite (SASOL SCF-55 from Sasol) and ferric nitrate were added at levels of 1.0 wt% and 4.5 wt%, respectively, of the final calcined washcoat. Finally, beta zeolite in ammonium form and SAR value 25 was added and then the slurry was aged for two days.
b) The slurry was then coated onto a ceramic substrate having a 400cpsi/4.3 grind cell structure and a 4.66 inch round by 4.5 inch length, resulting in a total volume of 1.26 liters and 3.636g/in 3 Or 222g/l WC loading. Calcination of the coated traps was done in air at 540 ℃.
c) After the trapping layer is applied in step b), a thin coating of a Three Way Catalyst (TWC) layer is applied. The washcoat loading of TWC layer was 1.5g/in 3 And a platinum group metal loading of 10g/ft 3 Wherein Pt: pd, rh=0:1:1.
The catalyst obtained was designated CC1.
Example 1
The catalyst of the present invention was prepared as described in example 1, but in this case, the Pd solution tape was applied by immersing one end of the catalyst in a Pd nitrate solution comprising citric acid and 2 wt% ethanol. The substrate used was 400cpsi/4.3 grind cell configuration, 4.66 inch round by 4.5 inch long, resulting in a total volume of 1.26 liters. The concentration of the impregnation solution was adjusted so that the Pd concentration in the impregnation zone was 250g/ft with a solution belt length of 3cm (1.2 inches) 3 . Average PGM loading over the whole fraction was 60g/ft at 0:11:1 3 (Pd is included in the band and in the TWC layer).
The catalyst obtained is called C1
Comparison of comparative example 1 and example 1
a) CC1 and C1 both have the same three-way catalyst washcoat and the same 10g/ft 3 Wherein Pt: pd: rh=0:1:1, the only difference being the presence of a Pd band at the outlet of C1.
b) Prior to testing, catalysts CC1 and C1 were conditioned for 2 hours in 4-mode 60 seconds cycle as follows:
the engine is operated at a speed load to produce an exhaust gas mass flow of 50 + -2.5 g/s per converter.
Catalyst inlet temperature (inlet) 1560.+ -. 10 ℃ F. (mode 1) during steady state
For mode 3, will O 2 Set to 4.5±0.1%. Since the flow balance is completed just before the aging starts, O 2 The concentration may not be exactly the same for all four branches. Furthermore, only one branch was used to measure the 4.5±0.1% oxygen level in mode 3.
For mode 2, CO was set to 4.0±0.1%, and for mode 3, CO was set to 2.5±0.1%.
4-mode 60 second cycle:
mode 1:40s @ lambda = 1.000 with no secondary air injection
Mode 2:6s@4% CO (enrichment), no secondary air injection
Mode 3:10s@2.5%CO (enrichment), secondary air injection is opened
Mode 4:4s @ lambda=1.000, and secondary air injection is on
c) After conditioning catalysts CC1 and C1, the following aging was carried out for 23 hours:
the engine is operated at a speed load to produce an exhaust gas mass flow of 47±2.5g/s per converter.
Procatalyst bed temperature (F bed) 1580.+ -. 10°F during steady state (mode 1)
Catalyst pre-bed temperature during peak (F-bed) 1740.+ -. 10. Degree. F (mode 3)
For mode 3, will O 2 Set to 4.5±0.1%. Since the flow balance is completed just before the aging starts, O 2 The concentration may not be exactly the same for all four branches. Furthermore, only one branch was used to measure the 4.5±0.1% oxygen level in mode 3.
For mode 2, CO was set to 4.0±0.1%, and for mode 3, CO was set to 2.5±0.1%.
If the peak does not reach 1740.+ -. 10 ℃ F, then O is first taken 2 Reduced to a minimum of 3.2 + -0.1%
If the peak has not reached 1740+ -10 DEG F, then increasing the CO of mode 3 to a maximum of 3.0+ -0.1%
4-mode 60 second cycle:
mode 1:40s @ lambda = 1.000 with no secondary air injection
Mode 2:6s@4% CO (enrichment), no secondary air injection
Mode 3:10s@2.5%CO (enrichment), secondary air injection is opened
Mode 4:4s @ lambda=1.000, and secondary air injection is on
d) The light-off temperatures (T) of the conditioned and aged catalysts CC1 and C1 were determined as follows 50 -value): for testing, a Ford 4.6L MPFI engine operating at 1700RPM was used. GHSV was set at 35K and was performed at 51℃per minute
Figure BDA0002781642420000091
Is provided for the temperature ramp of (a). During the temperature ramp, λ was set to 1.00±0.045@1hz. The fuel used was indole transparent and contained 20ppm sulfur.
The following results were obtained:
Figure BDA0002781642420000092
e) The overall% conversion of HC in lambda traversal tests of conditioned and aged catalysts CC1 and C1 at 450, 500, and 600 ℃ was determined as follows. For the 450 ℃ lateral test, a Ford 4.6L MPFI engine operating at 1700RPM was used. GHSV was set at 70K and 1.044/lean was performed in 458 seconds
Figure BDA0002781642420000093
0.948/enriched continuous lambda scan. λ=1.00±0.045@1hz at stoichiometry. The fuel used was indole transparent with 20ppm sulfur. Based on the conversion between λ1.01 and 0.99, the "overall property value" of each component is calculated. 500 ℃ testing differs from 450 ℃ scanning in that it is done in a 680 second period and lambda at stoichiometry is 1.00 ± 0.055@1hz. The 600 ℃ scan was completed under the same conditions as the 500 ℃ scan, except for the higher temperature.
The following results were obtained:
Figure BDA0002781642420000094
comparative example 2
Comparative example 1 was repeated, with the only difference that the PGM content of the TWC layer was higher and the TWC layer was composed of pd+rh=50g/ft 3 Composition @ 0:10:1. The catalyst obtained is called CC2.
Example 2
The catalyst of the present invention was prepared as described in comparative example 2 above, except that in this case pd=25 g/ft 3 Is added to the trapping layer to give a uniform distribution over the entire length of the portion. All Rh was treated at 5g/ft 3 Added to the TWC layer. The remaining Pd was then applied as a short band by immersing one end of the catalyst in a Pd nitrate solution containing citric acid and 2 wt% ethanol. The target tape length was 0.5 inches. The concentration of the impregnation solution was adjusted so that the total Pd concentration in the impregnation zone was 250g/ft with a solution belt length of 1.25cm (0.5 inch) 3 . Average PGM loading over the whole fraction was 55g/ft at 0:10:1 3 (Pd was included in the belt and in the trapping layer). The catalyst obtained is called C2.
Comparison of comparative example 2 and example 2
The catalyst was aged using a 2-hour 4-mode preconditioning step followed by a 23-hour 4-mode aging step in the presence of P in the fuel, as described above. Testing was performed using the procedure as described by Nunan et al. SAE 2013-01-1297. The results are summarized in fig. 2, where the total HC emissions of both CC2 and C2 are compared. It is evident that the catalyst of the present invention with Pd-bands at the rear has lower trapping emissions for both the initial adsorption step in the temperature range of 30-55 ℃ and the high T-release of strongly bound HC in the temperature range of 230-330 ℃. Thus, the presence of Pd bands at the rear has improved HC adsorption and improved conversion at higher temperatures, resulting in reduced HC emissions.

Claims (18)

1. A catalyst comprising a length L of a carrier substrate extending between a substrate end a and a substrate end B and two washcoat zones a and B, wherein
The washcoat zone A comprises a compound of a redox-active base metal selected from Cu, ni, co, mn, fe, cr, ce, pr, tb, sn and In supported on zeolite and/or on a support oxide and palladium and extends over a portion of the length L from the substrate end a, and
the washcoat zone B comprises the same composition and additional amounts of palladium as the washcoat zone a and extends from the substrate end B over a portion of the length L,
wherein l=l A +L B Wherein L is A Length of the wash coat zone A and L B Is the length of the wash-coated region B, and
wherein the catalyst comprises zeolite in washcoat zones a and B in an amount of 120g/l to 340g/l based on the volume of the support substrate.
2. The catalyst of claim 1, wherein
The washcoat zone A comprises two layers A1 and A2, both of which layers A1 and A2 are at the length L A Upper extension, wherein layer A1 comprises a compound of a redox-active base metal selected from Cu, ni, co, mn, fe, cr, ce, pr, tb, sn and In supported on a zeolite and palladium, and layer A2 comprises rhodium, and
the washcoat zone B comprises two layers B1 and B2, both layers B1 and B2 being at the length L B Upper extension, wherein layer B1 comprises the same composition as layer A1 and layer B2 comprises the same composition as layer A2, and wherein layers B1 and B2 comprise an additional amount of palladium compared to layers A1 and A2.
3. The catalyst of claim 1 or 2, wherein washcoat zone a and B are identical except for a greater amount of palladium contained in washcoat zone B.
4. The catalyst of claim 1 or 2, wherein the redox active base metal is copper, manganese or iron.
5. The catalyst of claim 4, wherein the redox active base metal is iron.
6. The catalyst of claim 1 or 2, wherein the redox active base metal is present as a cation or as an oxide.
7. The catalyst of claim 5, wherein the catalyst is based on the volume of the support substrate and is in Fe 2 O 3 The calculations were performed with the catalyst comprising iron compounds in the washcoat zones A and B in an amount of 1.0g/l to 30 g/l.
8. The catalyst of claim 1 or 2, wherein the zeolite belongs to structure type code BEA, FAU, FER, MFI or MOR.
9. The catalyst of claim 1 or 2, wherein the zeolite is a beta zeolite.
10. The catalyst of claim 5 wherein the redox active base metal compound and palladium in washcoat zone a are supported on the zeolite.
11. The catalyst of claim 10, wherein the redox active base metal and palladium are present in the zeolite structure as cations or in the zeolite and/or on the surface of the zeolite as oxides and metals, respectively.
12. The catalyst of claim 1 or 2, wherein the support oxide is alumina, silica, magnesia, titania, ceria, zirconia, or a mixture or mixed oxide comprising at least two of these materials.
13. The catalyst of claim 1 or 2, wherein palladium is present in cationic, metallic or oxide form.
14. The catalyst of claim 1 or 2, wherein the catalyst comprises palladium in the washcoat zone a in an amount of 0.04g/l to 4.0g/l based on the volume of the support substrate and calculated as palladium metal.
15. The catalyst of claim 1 or 2, wherein the catalyst comprises palladium in the washcoat zone B in an amount of 2g/l to 20g/l based on the volume of the support substrate and calculated as palladium metal.
16. The catalyst of claim 1 or 2, wherein washcoat zone a extends over 70% to 95% of the length L of the carrier substrate and washcoat zone B extends over 5% to 30% of the length L of the carrier substrate.
17. The catalyst of claim 1 or 2, wherein the carrier substrate of the length L is a flow-through substrate or a filter substrate.
18. A method of treating exhaust gas of a combustion engine, wherein the exhaust gas passes over the catalyst of any one of claims 1 to 17, wherein the exhaust gas enters the catalyst at substrate end a and exits the catalyst at substrate end b.
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